The UV laser properties of trivalent cerium-doped LiSrAlF6 (Ce:LiSAF) and LiCaAlF6 (Ce:LiCAF) are reported. The polarized absorption, emission, and excited-state absorption cross sections for both Ce:LiSAF and Ce:LiCAF were determined for the 266-nm pump and 290-nm laser emission wavelengths. The single-exponential emission lifetime was measured to be 28 ± 2 and 25 ± 2 ns for Ce:LiSAF and Ce:LiCAF, respectively. The gain was found to be highest when the probe was polarized parallel to the optical axis of the crystal, owing to the anisotropic nature of the excited-state absorption. The excited-state absorption was ascribed to a transition from the 5d orbital of Ce3+ to the conduction band of the host. Laser slope efficiencies as high as 29% and 21%, respectively, were measured for Ce:LiSAF and Ce:LiCAF when the 266-nm pulsed pump beam was polarized parallel to the optical or the c axis. These are the highest laser slope efficiencies yet observed to our knowledge for any known solid-state UV laser material. When the pump beam was polarized perpendicular to the optical axis of the crystals, the gain and the laser efficiencies dropped by as much as an order of magnitude. The magnitude of pump-induced solarization was found to be highly variable for different crystals and to have an insignificant effect on the laser performance when favorable crystals were used.
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